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Low-potential-driven electrocatalytic reduction of CO2 to hydrocarbons by cobalt-based metal-organic nanosheets
Journal of Catalysis ( IF 7.3 ) Pub Date : 2022-06-15 , DOI: 10.1016/j.jcat.2022.06.018
Bing Shao , Xin Chen , Yan-Tong Xu , Guo-Qing Li , Jing-Ping Zhong , Ting Meng , Zhong Zhang , Fu-Ping Huang , Jin Huang

The CO2 reduction reaction products of Co-based electrocatalysts are mainly CO and HCOOH, but there are few reports on hydrocarbons with the highest added value. Herein, a novel Co-based MOFs with V-type trinuclear cluster was constructed and exfoliated by ultrasound into ultrathin metal–organic nanosheets (∼3 nm) that retain the precursor structure. The Cobalt-based metal-organic nanosheets exhibits an excellent electrocatalytic reduction of CO2 performance with the relatively low overpotential of −0.4 V at the current density of 8.4 mA cm−2 and the Faradaic efficiency of CH4 and C2H6 is 22.4 % and 11.6 %, respectively. The in-situ Raman spectroscopy and density functional theory calculations indicate that the catalytic sites of Co at both ends of the V-type cluster more easily convert *CO into intermediates of *COH therefore formation the removable *CH3, and they can be reduced to CH4 or coupled form C2H6 in the process of shedding and the environment of hydrogen evolution reaction.



中文翻译:

钴基金属有机纳米片低电位驱动电催化还原 CO2 为碳氢化合物

Co基电催化剂的CO 2还原反应产物主要是CO和HCOOH,但关于附加值最高的碳氢化合物的报道较少。在此,构建了一种具有 V 型三核簇的新型 Co 基 MOF,并通过超声剥离成超薄金属有机纳米片(~3 nm),该纳米片保留了前体结构。钴基金属有机纳米片表现出优异的CO 2电催化还原性能,在8.4 mA cm -2的电流密度下具有-0.4 V相对较低的过电位, CH 4和C 2 H 6的法拉第效率为22.4 % 和 11.6%,分别。现场拉曼光谱和密度泛函理论计算表明,V型簇两端的Co催化位点更容易将*CO转化为*COH的中间体,从而形成可去除的*CH 3,它们可以还原为CH 4或在脱落过程和析氢反应环境中偶联形成C 2 H 6 。

更新日期:2022-06-15
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